Multiple iodide autocatalysis paths of chemo-hydrodynamical patterns in the Briggs–Rauscher reaction

自催化 碘化物 化学 催化作用 计算化学 有机化学 物理
作者
Lei Yuan,Hongzhang Wang,Chen Meng,Zhenfang Cheng,Xiaoli Lv,Qingyu Gao
出处
期刊:Physical Chemistry Chemical Physics [Royal Society of Chemistry]
卷期号:25 (18): 13183-13188
标识
DOI:10.1039/d3cp00011g
摘要

Autocatalytic feedback is often regarded as the core step for the chemo-hydrodynamical patterns in the nonlinear reaction system. The Briggs-Rauscher (BR) reaction shows sequential chemo-hydrodynamical patterns with three states, i.e. labyrinth, high iodine state, and rotating dendritic patterns. The short-lived labyrinth patterns, depending on [Mn2+]0, the ratio of [CH2(COOH)2]0 and [KIO3]0 and light intensities, result from iodide autocatalytic loop, which has three paths (involving Mn2+-induced radical reactions, the oxidation of iodomalonic compounds, and light-induced radical reactions, respectively). The high iodine state appears in a high ratio of [CH2(COOH)2]0 and [KIO3]0, relating to the autocatalytic path involving the oxidation of iodomalonic compounds. The light-induced radical autocatalytic path can act as a convenient control parameter to modulate the patterns in the first stage by increasing the iodine radicals. The dendritic patterns in the third stage result from the Marangoni effect caused by the evaporation of the solutions and reactions between H2O2 and iodine-containing species, which is independent of [CH2(COOH)2]0 and [Mn2+]0. This work contributes to a better understanding of the complex spatiotemporal patterns in the chemo-hydrodynamical system.
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